Observation of unstable reaction intermediate by picosecond tunable infrared laser pulses

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The picosecond tunable infrared laser pulses enabled us to carry out the vibrational spectroscopic measurements of the species adsorbed on surfaces with picosecond time-resolution. The irradiation of near-infrared pump pulses causes thermal excitation of the surface, and the change of adsorbates was probed by sum-frequency generation (SFG) spectroscopy. We applied this method to the direct observation of unstable species of formate on NiO(111) surface. The stable bidentate formate on NiO(111) was transformed to monodentate by the irradiation of pump pulses, and the dynamic behavior of the newly observed monodentate formate was followed as a precursor for the decomposition of formate. The application of the present method has extended to the study of methoxy species on Ni(111).

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